On November 1, 1897, the new Library of Congress building opened its doors to the public. Previously, the Library had been housed in the Congressional Reading Room in the U.S. Capitol. In the twentieth century, two additional buildings were added to the Library of Congress complex on Capitol Hill.

In 1871, Librarian of Congress Ainsworth Spofford first suggested the construction of a separate building for the Library, which had outgrown its cramped quarters. According to Library historian John Y. Cole, Spofford envisioned "a circular, domed reading room at the Library's center, surrounded by ample space for the Library's various departments." After much debate and two design competitions, Congress finally approved the plan in 1886, designed in the Italian Renaissance style by Washington architects John L. Smithmeyer and Paul J. Pelz. The building was an important step towards Spofford's overall goal of establishing the Library of Congress as an American national library. When completed, it was the largest and costliest library building in the world.

Brigadier General Thomas Lincoln Casey and Bernard R. Green of the U.S. Army Corps of Engineers assumed control of the project in 1888. They soon began to focus on the interior of the building, which they hoped to make a showcase for the talents of American artists and artisans. "The elaborate embellishment" of the building's interior, writes Cole in Jefferson's Legacy, "is worth careful attention, for few structures represent human thought and aspiration in such dramatic fashion."

In 1980, the building was renamed the Thomas Jefferson Building in honor of the nation's third president. Jefferson sold his personal collection of 6,487 books to the Library of Congress in 1815, after its holdings were destroyed when the British burned the Capitol during the War of 1812. Jefferson’s wide-ranging interests as reflected in his books decisively expanded the scope of the Library’s mission. Today, Thomas Jefferson's Library continues to be available for the use of researchers, but it is also displayed for visitors to the Library's exhibit halls in the Jefferson Building, and on the World Wide Web.

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